US20050124788A1 - Intermediates for lhrh antagonist synthesis, process for their production, and process for lhrh antagonist production - Google Patents

Intermediates for lhrh antagonist synthesis, process for their production, and process for lhrh antagonist production Download PDF

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Publication number
US20050124788A1
US20050124788A1 US10/500,047 US50004705A US2005124788A1 US 20050124788 A1 US20050124788 A1 US 20050124788A1 US 50004705 A US50004705 A US 50004705A US 2005124788 A1 US2005124788 A1 US 2005124788A1
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US
United States
Prior art keywords
boc
4clphe
heptapeptide
3pal
lys
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Abandoned
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US10/500,047
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English (en)
Inventor
Jon Rasmussen
Palle Rasmussen
Wolfgang Wachs
Stefan Hansen
Jens Fomsgaard
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Polypeptide Laboratories AS
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Individual
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Assigned to POLYPEPTIDE LABORATORIES A/S reassignment POLYPEPTIDE LABORATORIES A/S ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: RASMUSSEN, JON H., RASMUSSEN, PALLE H., WACHS, WOLFGANG O., FOMSGAARD, JENS, HANSEN, STEFAN
Publication of US20050124788A1 publication Critical patent/US20050124788A1/en
Priority to US12/189,925 priority Critical patent/US8173770B2/en
Abandoned legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07KPEPTIDES
    • C07K5/00Peptides containing up to four amino acids in a fully defined sequence; Derivatives thereof
    • C07K5/04Peptides containing up to four amino acids in a fully defined sequence; Derivatives thereof containing only normal peptide links
    • C07K5/08Tripeptides
    • C07K5/0802Tripeptides with the first amino acid being neutral
    • C07K5/0804Tripeptides with the first amino acid being neutral and aliphatic
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07KPEPTIDES
    • C07K7/00Peptides having 5 to 20 amino acids in a fully defined sequence; Derivatives thereof
    • C07K7/04Linear peptides containing only normal peptide links
    • C07K7/23Luteinising hormone-releasing hormone [LHRH]; Related peptides
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07KPEPTIDES
    • C07K1/00General methods for the preparation of peptides, i.e. processes for the organic chemical preparation of peptides or proteins of any length
    • C07K1/02General methods for the preparation of peptides, i.e. processes for the organic chemical preparation of peptides or proteins of any length in solution
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07KPEPTIDES
    • C07K5/00Peptides containing up to four amino acids in a fully defined sequence; Derivatives thereof
    • C07K5/04Peptides containing up to four amino acids in a fully defined sequence; Derivatives thereof containing only normal peptide links
    • C07K5/08Tripeptides
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07KPEPTIDES
    • C07K5/00Peptides containing up to four amino acids in a fully defined sequence; Derivatives thereof
    • C07K5/04Peptides containing up to four amino acids in a fully defined sequence; Derivatives thereof containing only normal peptide links
    • C07K5/08Tripeptides
    • C07K5/0827Tripeptides containing heteroatoms different from O, S, or N

Definitions

  • the present invention relates to intermediates for the synthesis of LHRH antagonists, to a process for the production of these intermediates and to a process for the production of LHRH antagonists.
  • LHRH The luteinizing hormone-releasing hormone, LHRH, controls the secretion of follicle stimulating hormone (FSH) and luteinizing hormone (LH).
  • LHRH antagonists are compounds capable of blocking the secretion of FSH and LH. They are generally nona- and decapeptides (but may be shorter or longer) comprising part of or the entire structure of LHRH in which one or several amino acids have been exchanged for other natural amino acids and/or amino acids not found in nature.
  • Synthetic LHRH antagonists may be used for contraception and in the treatment of benign hyperplasia of the prostate gland, hormonal-dependent tumors of the breast and ovaries, dysmenorrhea, endometriosis, and other conditions.
  • These synthetic LHRH antagonists have the general formula Ac-D-2Nal-D-4ClPhe-D-3Pal-Ser-X—NH 2 , wherein X is from 5 to 6 natural and/or synthetic amino acid residues.
  • X is AA1-AA2-Leu-AA3-Pro-D-Ala, in particular wherein AA1 is a natural or synthetic amino acid and AA2 is a natural or synthetic amino acid or zero, AA3 is a natural or synthetic amino acid.
  • a synthesis strategy disclosed in U.S. Pat. No. 5,710,246 for making decapeptide or nonapeptide LHRH antagonists comprises the coupling of an intermediate tripeptide representing amino residues 1 to 3 (counting starts at the amino terminal of the peptide) with a heptapeptide or a hexapeptide, respectively representing amino acid residues 4-10 and 4-9, respectively.
  • the intermediate tripeptide disclosed in U.S. Pat. No. 5,710,246 A is an ester, Boc-D-2Nal-D-4ClPhe-D-3Pal-O-Me or the corresponding benzyl or allyl ester.
  • a tripeptide representing amino acids 1-3 of an LHRH antagonist the terminal amino group of which is Boc- or Ac-protected and the terminal carboxyl group of which (that is, the terminal group of amino acid no. 3) is not protected.
  • the tripeptide (I) in the synthesis of a peptide of the general formula (IIa) Ac-D-2Nal-D-4ClPhe-D-3Pal-Ser-AA1-AA2-Leu-Lys(iPr)-Pro-D-Ala-NH 2 (IIa), wherein AA1 and AA2 have the meaning given above, in particular a LHRH antagonist of the formula (III) Ac-D-2Nal-D-4ClPhe-D-3Pal-Ser-MeTyr-D-Lys(Nic)-Leu-Lys(iPr)-Pro-D-Ala-NH 2 (III) or, even more preferred, of the formula (IIIa) Ac-D-2Nal-D-4ClPhe-D-3Pal-Ser-MeTyr-D-Asn-Leu-Lys(iPr)-Pro-D-Ala-NH 2 (IIIa).
  • the process of the invention for preparing a LHRH antagonist comprises the step of coupling the tripeptide (I) with a heptapeptide (IV) of the general formula P 1 -Ser(P 2 )-AA1-AA2-Leu-Lys(iPr,P 4 )-Pro-D-AlaNH 2 (IV), wherein P 4 is H or an amino protecting group such as Boc, wherein AA1 and AA2 have the aforementioned meaning, in particular with a heptapeptide (V) of the general formula P 1 -Ser(P 2 )-NMeTyr(P 3 )-D-Lys(Nic)-Leu-Lys(iPr, P 4 )-Pro-D-AlaNH 2 (V), wherein P 1 is selected from H or amino protecting group and P 2 and P 3 are independently selected from H and —OH protecting group, and P 4 has the meaning given above, for preparing the LHRH antagonist Ac-D-2Nal-D-4Cl
  • the heptapeptide (V) is described in U.S. Pat. No. 5,710,246 A.
  • the heptapeptide of the general formula (IV) including the heptapeptide (Va) can be synthesized by routine modifications of the synthesis of (V) or by coupling the corresponding Boc-amino acids on a peptide synthesizer (Beckman Model 990), as described in WO 94/40757 where also the LHRH antagonist (III) is disclosed.
  • the process of the invention for preparing a LHRH antagonist comprises the step of coupling the tripeptide (IX) Boc-D-2Nal-D-4ClPhe-D-3Pal—OH (IX) with a heptapeptide (IV) of the general formula P 1 -Ser(P 2 )-AA1-AA2-Leu-Lys(iPr, P 4 )-Pro-D-AlaNH 2 (IV), wherein P 1 , P 2 , P 4 , AA1 and AA2 have the meaning given above, in particular with a heptapeptide (V) of the general formula P 1 -Ser(P 2 )-NMeTyr(P 3 )-D-Lys(Nic)-Leu-Lys(iPr, P 4 )-Pro-D-AlaNH 2 (V) or, even more preferred, with a heptapeptide of the general formula (Va) P 1 -Ser(P 2 )-NM
  • the heptapeptide of the general formula (V) is the heptapeptide (VI) H-Ser(tBu)-NMeTyr-D-Lys(Nic)-Leu-Lys(iPr,Boc)-Pro-D-AlaNH 2 (VI), or even more preferred, the heptapeptide (VIa) H-Ser(tBu)-NMeTyr-D-Asn-Leu-Lys(iPr,Boc)-Pro-D-AlaNH 2 (VIa)
  • a particular advantage with the method of the invention is that a cheaper starting material, H-D-Pal-OH.2HCl, can be used instead of the ester H-Pal-OR.2HCl; the protective group of the starting material need not be removed. Therefore the synthesis of the invention is one step shorter and avoids that material is lost in the additional step.
  • Another advantage is that the formation of impurities in the saponification step is avoided. The formation of such impurities is well known. For instance, the basic conditions at the ester hydrolysis step cause partial racemization of D-Pal.
  • the other prior-art alternative of removing the ester group by catalytic hydrogenation in the case of allyl or benzyl ester groups) risks to cause a loss of Cl from 4ClPhe producing Phe. While allyl groups may be removed by still other reagents the full removal is difficult to control.
  • Boc-D-4ClPhe-OSu Boc-D-4ClPhe-OH (299,75 g; 1,0 eq.) and HONSu (184,1 g; 1,6 eq.) are dissolved in 2-propanol (4,5 L). The mixture is cooled to 0° C. and DIC (164,1 g; 1.3 eq.) is added. The mixture is stirred for 16 h while warming to room temperature. The product is filtered of, washed with 2-propanol (1,5 L) and dried. Yield: 85%. HPLC purity: 98,8%.
  • Boc-D-4ClPhe-D-3Pal-OH H-D-3Pal-OH, 2 HCl (251,1 g; 1,05 eq.) and Boc-D-4ClPhe-OSu (396,8 g; 1,0 eq.) are dissolved in DMSO (3,33 L) and NMM (318,8 g; 3,15 eq.) is added. The mixture is stirred for 16 h at room temperature. Water (17 L) is added and pH is adjusted to 4-4,5 which causes the product to precipitate. The mixture is filtered and the product is washed with water (3 ⁇ 5 L) to remove traces of DMSO, H-D-3Pal-OH and Boc-D-4ClPhe-OH. The product is dried. Yield: 80%. HPLC purity: 97,8%
  • Boc-D-2Nal-OSu Boc-D-2Nal-OH (315,4 g; 1,0 eq.) is dissolved in 2-propanol (6,8 L) at ⁇ 10° C. and IBC (157 g; 1,15 eq.) and NMM (116 g; 1,15 eq.) is added. After stirring for 5-10 min a mixture of HONSu (230,1 g; 2,0 eq.) in 2-propanol (1,4 L) is added. Additional NMM (10,1 g; 0,1 eq.) is added. After half an hour water (0,82 L) is added to dissolve precipitated NMM ⁇ HCl. The product is isolated by filtration, washed with 2-propanol (1 L), and dried. Yield.: 90%. HPLC purity: 98,3%.
  • Boc-D-4ClPhe-D-3Pal-OH (447,93 g; 1,0 eq.) is dissolved in a mixture of ethyl acetate (3,4 L), acetic acid (675 ml) and MSA (454 mL; 7,0 eq.) at 0° C. and kept at this temperature for two hours.
  • TEA (1669 ml; 12 eq.) is added.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Proteomics, Peptides & Aminoacids (AREA)
  • Biophysics (AREA)
  • General Health & Medical Sciences (AREA)
  • Genetics & Genomics (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Molecular Biology (AREA)
  • Biochemistry (AREA)
  • Endocrinology (AREA)
  • Analytical Chemistry (AREA)
  • Peptides Or Proteins (AREA)
  • Medicines That Contain Protein Lipid Enzymes And Other Medicines (AREA)
  • Preparation Of Compounds By Using Micro-Organisms (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Nitrogen Condensed Heterocyclic Rings (AREA)
US10/500,047 2001-12-29 2002-12-23 Intermediates for lhrh antagonist synthesis, process for their production, and process for lhrh antagonist production Abandoned US20050124788A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
US12/189,925 US8173770B2 (en) 2001-12-29 2008-08-12 Intermediates for LHRH antagonist synthesis, process for the production, and process for LHRH antagonist production

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
SE0104463-5 2001-12-29
SE0104463A SE0104463D0 (sv) 2001-12-29 2001-12-29 Mellanprodukter för syntes af LHRH-antagonister, sätt att framställa dem och sätt för framställning av LHRH-antagonister
PCT/IB2002/005583 WO2003055902A1 (en) 2001-12-29 2002-12-23 Intermediates for lhrh antagonist synthesis, process for their production, and process for lhrh antagonist production

Related Child Applications (1)

Application Number Title Priority Date Filing Date
US12/189,925 Continuation US8173770B2 (en) 2001-12-29 2008-08-12 Intermediates for LHRH antagonist synthesis, process for the production, and process for LHRH antagonist production

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US20050124788A1 true US20050124788A1 (en) 2005-06-09

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US10/500,047 Abandoned US20050124788A1 (en) 2001-12-29 2002-12-23 Intermediates for lhrh antagonist synthesis, process for their production, and process for lhrh antagonist production
US12/189,925 Expired - Lifetime US8173770B2 (en) 2001-12-29 2008-08-12 Intermediates for LHRH antagonist synthesis, process for the production, and process for LHRH antagonist production

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US (2) US20050124788A1 (enExample)
EP (2) EP1465917B1 (enExample)
JP (1) JP4272529B2 (enExample)
KR (1) KR100844520B1 (enExample)
CN (1) CN1304417C (enExample)
AT (2) ATE371666T1 (enExample)
AU (1) AU2002348749B2 (enExample)
CA (1) CA2471723C (enExample)
CY (2) CY1107580T1 (enExample)
DE (2) DE60222189T2 (enExample)
DK (2) DK1465917T3 (enExample)
ES (2) ES2296050T3 (enExample)
IL (2) IL162788A0 (enExample)
NO (1) NO330129B1 (enExample)
NZ (1) NZ534245A (enExample)
PT (2) PT1630169E (enExample)
RU (1) RU2307125C2 (enExample)
SE (1) SE0104463D0 (enExample)
SI (1) SI1630169T1 (enExample)
WO (1) WO2003055902A1 (enExample)
ZA (1) ZA200405136B (enExample)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20090234098A1 (en) * 2004-03-09 2009-09-17 Ajinomoto Co., Inc. Method of preparing peptide

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101037472B (zh) * 2006-03-14 2013-03-27 中国人民解放军军事医学科学院毒物药物研究所 具有低组胺释放作用的促黄体生成素释放激素拮抗剂
JOP20090061B1 (ar) 2008-02-11 2021-08-17 Ferring Int Center Sa طريقة معالجة سرطان البروستاتا بمضادات الهرمونات التناسلية GnRH
DK2632934T3 (en) 2010-10-27 2017-01-23 Ferring Bv Process for the preparation of Degarelix and its intermediates
EP2447276A1 (en) 2010-10-27 2012-05-02 Ferring B.V. Process for the manufacture of Degarelix and its intermediates
PL4512389T1 (pl) 2012-06-01 2025-09-01 Ferring B.V. Produkt leczniczy degareliksu

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4098777A (en) * 1977-03-14 1978-07-04 Merck & Co., Inc. Process for the preparation of pyroglutamyl-Ala-Lys-Ser-Gln-Gly-Gly-Ser-Asn
US5322931A (en) * 1990-07-24 1994-06-21 Eastman Kodak Company Process for synthesizing peptides - fragment condensation
US5710246A (en) * 1996-03-19 1998-01-20 Abbott Laboratories Process for intermediates for the synthesis of LHRH antagonists
US6235734B1 (en) * 1996-10-30 2001-05-22 Pfizer Inc Pyridone-fused azabicyclic- or cytisine derivatives, their preparation and their use in addiction therapy
US6699833B1 (en) * 1996-12-11 2004-03-02 Praecis Pharmaceuticals, Inc. Pharmaceutical formulations for sustained drug delivery

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
SU1623166A1 (ru) * 1989-04-03 1994-02-15 Институт биоорганической химии АН БССР Нейтропептиды, обладающие поведенческой активностью
US5225598A (en) * 1990-03-30 1993-07-06 Union Carbide Chemicals & Plastics Technology Corporation Selective production of linear pentaethylenehexamine and hydroxyethyldiethylenetriamine
DE19941248A1 (de) 1998-09-01 2000-03-02 Asta Medica Ag Peptide mit N-substituierten Glycingruppen sowie diese enthaltende Arzneimittel zur Behandlung hormonabhängiger Tumore

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4098777A (en) * 1977-03-14 1978-07-04 Merck & Co., Inc. Process for the preparation of pyroglutamyl-Ala-Lys-Ser-Gln-Gly-Gly-Ser-Asn
US5322931A (en) * 1990-07-24 1994-06-21 Eastman Kodak Company Process for synthesizing peptides - fragment condensation
US5710246A (en) * 1996-03-19 1998-01-20 Abbott Laboratories Process for intermediates for the synthesis of LHRH antagonists
US6235734B1 (en) * 1996-10-30 2001-05-22 Pfizer Inc Pyridone-fused azabicyclic- or cytisine derivatives, their preparation and their use in addiction therapy
US6699833B1 (en) * 1996-12-11 2004-03-02 Praecis Pharmaceuticals, Inc. Pharmaceutical formulations for sustained drug delivery

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20090234098A1 (en) * 2004-03-09 2009-09-17 Ajinomoto Co., Inc. Method of preparing peptide
US7915224B2 (en) * 2004-03-09 2011-03-29 Ajinomoto Co., Inc. Method of preparing peptide

Also Published As

Publication number Publication date
SE0104463D0 (sv) 2001-12-29
JP2005516962A (ja) 2005-06-09
ATE371666T1 (de) 2007-09-15
HK1075052A1 (en) 2005-12-02
KR100844520B1 (ko) 2008-07-08
CY1107580T1 (el) 2013-03-13
DK1465917T3 (da) 2007-02-19
SI1630169T1 (sl) 2008-04-30
PT1465917E (pt) 2007-01-31
DE60222189T2 (de) 2008-06-19
AU2002348749A1 (en) 2003-07-15
NZ534245A (en) 2007-05-31
JP4272529B2 (ja) 2009-06-03
US8173770B2 (en) 2012-05-08
IL162788A (en) 2010-12-30
DK1630169T3 (da) 2008-01-02
PT1630169E (pt) 2007-12-06
EP1465917B1 (en) 2006-10-18
CY1107025T1 (el) 2012-09-26
DE60222189D1 (de) 2007-10-11
IL162788A0 (en) 2005-11-20
RU2004119964A (ru) 2006-01-10
US20080306242A1 (en) 2008-12-11
NO20043047L (no) 2004-08-30
EP1630169A2 (en) 2006-03-01
NO330129B1 (no) 2011-02-21
RU2307125C2 (ru) 2007-09-27
WO2003055902A1 (en) 2003-07-10
KR20040090965A (ko) 2004-10-27
ZA200405136B (en) 2005-07-27
EP1465917A1 (en) 2004-10-13
ES2275012T3 (es) 2007-06-01
CN1622954A (zh) 2005-06-01
CA2471723A1 (en) 2003-07-10
CN1304417C (zh) 2007-03-14
EP1630169A3 (en) 2006-03-15
ATE342913T1 (de) 2006-11-15
EP1630169B1 (en) 2007-08-29
DE60215544D1 (de) 2006-11-30
ES2296050T3 (es) 2008-04-16
CA2471723C (en) 2011-02-15
DE60215544T2 (de) 2007-08-30
AU2002348749B2 (en) 2008-09-04

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Free format text: ASSIGNMENT OF ASSIGNORS INTEREST;ASSIGNORS:RASMUSSEN, JON H.;RASMUSSEN, PALLE H.;WACHS, WOLFGANG O.;AND OTHERS;REEL/FRAME:016247/0689;SIGNING DATES FROM 20041109 TO 20041205

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